A novel bilayer heterogeneous poly(ionic liquid) electrolyte for high-performance flexible supercapacitors with ultraslow self-discharge.

Flexible supercapacitors with high power density and long cyclic stability represent a promising candidate to be used as power supplies for portable electronics, but often suffer from the disadvantages of a limited working voltage and rapid self-discharge (spontaneous drop of open-circuit voltage). Here, we design a bilayer heterogeneous poly(ionic liquid) electrolyte (BHPE) consisting of a polycation complex and a polyanion complex with different zeta potentials to suppress the self-discharge of flexible symmetric supercapacitors. The resultant BHPE-based supercapacitors using active carbon/carbon nanotube composite electrodes exhibit a high working potential of 3.0 V and an energy density of 33 W h kg ^-1 , which are comparable with those of devices obtained by using a homogeneous poly(ionic liquid) electrolyte (HPE). More significantly, the developed BHPE-based supercapacitor charged under forward bias exhibits a self-discharge time of 23.2 h, which is at least twice that of the device charged under reverse bias and is also much superior to those of HPE-based supercapacitors. The BHPE-based supercapacitors also possess excellent mechanical flexibility and stability, due to the stabilized interface contact between two layers of poly(ionic liquid)s.